Shumin Zhang , Yaqi Wang , Zelin Wang , Libo Wang , Changsheng An , Difa Xu
{"title":"ZIS1−x/UCN S-scheme界面的超快电子转移实现了高效的H2O2光合作用和四环素降解","authors":"Shumin Zhang , Yaqi Wang , Zelin Wang , Libo Wang , Changsheng An , Difa Xu","doi":"10.1016/j.actphy.2025.100136","DOIUrl":null,"url":null,"abstract":"<div><div>Coupling H<sub>2</sub>O<sub>2</sub> production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn<sub>2</sub>S<sub>4</sub>/g-C<sub>3</sub>N<sub>4</sub> (ZIS<sub>1−<em>x</em></sub>/UCN) S-scheme heterojunction photocatalyst was constructed by <em>in situ</em> growing ZIS<sub>1−<em>x</em></sub> nanosheets on porous ultrathin UCN. The designed ZIS<sub>1−<em>x</em></sub>/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS<sub>1−<em>x</em></sub>/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H<sub>2</sub>O<sub>2</sub> production rate of 2902.2 μmol g<sup>−1</sup> h<sup>−1</sup> and 91.3 % tetracycline (50 mg L<sup>−1</sup>) degradation efficiency. This H<sub>2</sub>O<sub>2</sub> performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 μmol g<sup>−1</sup> h<sup>−1</sup>). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), <em>in situ</em> irradiation X-ray photoelectron spectroscopy (ISI-XPS), and <em>in situ</em> X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.</div></div>","PeriodicalId":6964,"journal":{"name":"物理化学学报","volume":"41 11","pages":"Article 100136"},"PeriodicalIF":13.5000,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation\",\"authors\":\"Shumin Zhang , Yaqi Wang , Zelin Wang , Libo Wang , Changsheng An , Difa Xu\",\"doi\":\"10.1016/j.actphy.2025.100136\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Coupling H<sub>2</sub>O<sub>2</sub> production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn<sub>2</sub>S<sub>4</sub>/g-C<sub>3</sub>N<sub>4</sub> (ZIS<sub>1−<em>x</em></sub>/UCN) S-scheme heterojunction photocatalyst was constructed by <em>in situ</em> growing ZIS<sub>1−<em>x</em></sub> nanosheets on porous ultrathin UCN. The designed ZIS<sub>1−<em>x</em></sub>/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS<sub>1−<em>x</em></sub>/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H<sub>2</sub>O<sub>2</sub> production rate of 2902.2 μmol g<sup>−1</sup> h<sup>−1</sup> and 91.3 % tetracycline (50 mg L<sup>−1</sup>) degradation efficiency. This H<sub>2</sub>O<sub>2</sub> performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 μmol g<sup>−1</sup> h<sup>−1</sup>). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), <em>in situ</em> irradiation X-ray photoelectron spectroscopy (ISI-XPS), and <em>in situ</em> X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.</div></div>\",\"PeriodicalId\":6964,\"journal\":{\"name\":\"物理化学学报\",\"volume\":\"41 11\",\"pages\":\"Article 100136\"},\"PeriodicalIF\":13.5000,\"publicationDate\":\"2025-07-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"物理化学学报\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S100068182500092X\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"物理化学学报","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S100068182500092X","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Ultrafast electron transfer at the ZIS1−x/UCN S-scheme interface enables efficient H2O2 photosynthesis coupled with tetracycline degradation
Coupling H2O2 production with organic pollutant degradation can effectively overcome the sluggish kinetics of water oxidation while concurrently addressing environmental pollution challenges. In this work, an S-defect-rich ZnIn2S4/g-C3N4 (ZIS1−x/UCN) S-scheme heterojunction photocatalyst was constructed by in situ growing ZIS1−x nanosheets on porous ultrathin UCN. The designed ZIS1−x/UCN photocatalyst demonstrates enhanced visible light absorption, abundant active sites, and intimate interfacial contact. The optimized ZIS1−x/UCN-1.0 photocatalyst exhibits outstanding dual functionality, simultaneously achieving an H2O2 production rate of 2902.2 μmol g−1 h−1 and 91.3 % tetracycline (50 mg L−1) degradation efficiency. This H2O2 performance represents a 1.63-fold enhancement compared to its activity in pure water (1777.0 μmol g−1 h−1). Through comprehensive characterization including femtosecond transient absorption spectroscopy (fs-TAS), in situ irradiation X-ray photoelectron spectroscopy (ISI-XPS), and in situ X-ray absorption fine structure spectroscopy (XAFS), we unequivocally confirm the S-scheme charge transfer mechanism. This S-scheme induced unique electronic structure not only fosters ultrafast electron transfer at the interface (3.54 ps) but also significantly enhances the redox capacity of photogenerated carriers. Collectively, this work opens new avenues for the dual application of photocatalytic technology in both energy production and environmental remediation.